A class of graphene oxide (GO) Ormosil glasses with excellent nonlinear optical properties were made with sol-gel method. The as-prepared GO Ormosil glasses were highly transparent in visible and near-infrared region, due to the uniform dispersion of modified GO in the matrix. These Ormosil glasses have a broadband optical limiting effect from 532 to 1570 nm, with lower optical limiting onset energy density (F ON ). The nonlinear absorption coefficients of the Ormosil glass could reach 210.62, 647.96, and 43.10 cm GW −1 at 532, 1064, and 1570 nm. The optical limiting properties of the Ormosil glasses come from nonlinear absorption proved by Z-scan measurements. Therefore, the Ormosil glasses have potential applications in nonlinear optical areas.